1. Scope -is the work directly or implicitly related to atmospheric composition? 2. Novelty -does the work provide a) a general and/or broader relevance (e.g. not a pure local study), b) new results or methods, and c) does it add significantly to the knowledge of atmospheric composition and its impacts?3. Quality -does the work contain high quality a) atmospheric observations, b) process studies, c) modeling exercises or d) data analysis?Will your paper be within the scope of Atmospheric Environment?We try to be flexible with novel scientific articles on issues of atmospheric composition even, if they are not directly related to atmospheric measurements (e.g. wind tunnel studies, dynamometer studies, remote sensing retrieval, etc). However, we are still cautious of purely mathematical derivations, preliminary results or insignificant case and local studies. The authors should make sure that the articles contain substantial contributions to the science of atmospheric composition before sending them for review.

[1] In this paper we present simulations with a Lagrangian particle dispersion model to study the intercontinental transport of pollution from North America during an aircraft measurement campaign over Europe. The model was used for both the flight planning and a detailed source analysis after the campaign, which is described here with examples from two episodes. Forward calculations of emission tracers from North America, Europe, and Asia were made in order to understand the transport processes. Both episodes were preceded by stagnant conditions over North America, leading to the accumulation of pollutants in the North American boundary layer. Both anthropogenic sources and, to a lesser extent, forest fire emissions contributed to this pollution, which was then exported by warm conveyor belts to the middle and upper troposphere, where it was transported rapidly to Europe. Concentrations of many trace gases (CO, NO y , CO 2 , acetone, and several volatile organic compounds; O 3 in one case) and of ambient atmospheric ions measured aboard the research aircraft were clearly enhanced in the pollution plumes compared to the conditions outside the plumes. Backward simulations with the particle model were introduced as an indispensable tool for a more detailed analysis of the plume's source region. They make trajectory analyses (which, to date, were mainly used to interpret aircraft measurement data) obsolete. Using an emission inventory, we could decompose the tracer mixing ratios at the receptors (i.e., along the flight tracks) into contributions from every grid cell of the inventory. For both plumes we found that emission sources contributing to the tracer concentrations over Europe were distributed over large areas in North America. In one case, sources in California, Texas, and Florida contributed almost equally, and smaller contributions were also made by other sources located between the Yucatan Peninsula and Canada. In the other case, sources in eastern North America, including moderate contributions from forest fires, were most important. The plume's maximum was mainly caused by anthropogenic emissions from the New York area. To our knowledge, this is the first case reported where a pollution plume from a megacity was reliably detected over another continent.

[1] A case of long-range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North America, the North Atlantic and Europe by three different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NO y , mainly in form of PAN. Observed O 3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, was used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume was investigated using in situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast-J), run in the model. Significant impacts on photochemistry are found with a decrease of 18% in O 3 production and 24% in O 3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O 3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O 3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O 3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutant levels in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales (averaging 6.25 days) were derived from CO changes. Observed and simulated O 3 /CO correlations in the plume were also compared in order to evaluate the photochemistry in the model. Observed slopes change from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting a small underestimation in modeled photochemical O 3 production. The possible impact of this biomass burning plume on O 3 levels in the European boundary layer was also examined by running the model for a further 5 days and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O 3 increases and elevated CO levels. The model predicts significant changes in O 3 over the entire 10 day period due to photochemistry but the signal is largely lost because of the effects of dilution. However, measurements in several other BB plumes over Europe show that O 3 impact of Alaskan fires can be potentially significant over Europe.

Abstract.Lightning is an important source of NO x in the free troposphere, especially in the tropics, with strong impact on ozone production. However, estimates of lightning NO x (LNO x ) production efficiency (LNO x per flash) are still quite uncertain.In this study we present a systematic analysis of NO 2 column densities from SCIAMACHY measurements over active thunderstorms, as detected by the World-Wide Lightning Location Network (WWLLN), where the WWLLN detection efficiency was estimated using the flash climatology of the satellite lightning sensors LIS/OTD. Only events with high lightning activity are considered, where corrected WWLLN flash rate densities inside the satellite pixel within the last hour are above 1 /km 2 /h. For typical SCIAMACHY ground pixels of 30 × 60 km 2 , this threshold corresponds to 1800 flashes over the last hour, which, for literature estimates of lightning NO x production, should result in clearly enhanced NO 2 column densities.From 2004-2008, we find 287 coincidences of SCIA-MACHY measurements and high WWLLN flash rate densities. For some of these events, a clear enhancement of column densities of NO 2 could be observed, indeed. But overall, the measured column densities are below the expected values by more than one order of magnitude, and in most of the cases, no enhanced NO 2 could be found at all.Our results are in contradiction to the currently accepted range of LNO x production per flash of 15 (2-40) × 10 25 molec/flash. This probably partly results from the specific conditions for the events under investigation, i.e. events of high lightning activity in the morning (local time) and mostly (for 162 out of 287 events) over ocean.Within the detected coincidences, the highest NO 2 column densities were observed around the US Eastcoast. This might Correspondence to: S. Beirle (steffen.beirle@mpic.de) be partly due to interference with ground sources of NO x being uplifted by the convective systems. However, it could also indicate that flashes in this region are particularly productive.We conclude that current estimates of LNO x production might be biased high for two reasons. First, we observe a high variability of NO 2 for coincident lightning events. This high variability can easily cause a publication bias, since studies reporting on high NO x production have likely been published, while studies finding no or low amounts of NO x might have been rejected as errorneous or not significant. Second, many estimates of LNO x production in literature have been performed over the US, which is probably not representative for global lightning.

[1] In situ measurements of formaldehyde (CH 2 O) onboard four European research aircraft in August 2006 as part of the African Monsoon Multidisciplinary Analysis (AMMA) experiment in West Africa are used (1) to examine the redistribution of CH 2 O by mesoscale convective systems (MCS) in the tropical upper troposphere (UT), (2) to evaluate the scavenging efficiency (SE) of CH 2 O by MCS and (3) to quantify the impact of CH 2 O on UT photooxidant production downwind of MCS. The intercomparison of CH 2 O measurements is first tested, providing a unique and consistent 3-D-spatially resolved CH 2 O database in background and convective conditions. While carbon monoxide (CO) is vertically uplifted by deep convection up to 12 km, CH 2 O is also affected by cloud processing as seen from its ratio relative to CO with altitude. A new observation-based model is established to quantify the SE of CH 2 O. This model shows that convective entrainment of free tropospheric air cannot be neglected since it contributes to 40% of the convective UT air. For the 4 studied MCS, SE shows a large variability within a 4% to 39% range at a relative standard deviation of 30%, which is consistent with MCS features. A time-dependent photochemical box model is applied to convective UT air. After convection, 60% of CH 2 O is due to its photochemical production rather than to its direct transport. Model results indicate that CH 2 O directly injected by convection does not impact ozone and HOx production in the tropical UT of West Africa. NOx and anthropogenic hydrocarbon precursors dominate the secondary production of CH 2 O, ozone and HOx.

Abstract. In the summer 2000 EXPORT aircraft campaign (European eXport of Precursors and Ozone by long-Range Transport), two comprehensively instrumented research aircraft measuring a variety of chemical species flew wing tip to wing tip for a period of one and a quarter hours. During this interval a comparison was undertaken of the measurements of nitrogen oxide (NO), odd nitrogen species (NO y ), carbon monoxide (CO) and ozone (O 3 ). The comparison was performed at two different flight levels, which provided a 10-fold variation in the concentrations of both NO (10 to 1000 parts per trillion by volume (pptv)) and NO y (200 to over 2500 pptv). Large peaks of NO and NO y observed from the Falcon 20, which were at first thought to be from the exhaust of the C-130, were also detected on the 4 channel NO xy instrument aboard the C-130. These peaks were a good indication that both aircraft were in the same air mass and that the Falcon 20 was not in the exhaust plume of the C-130. Correlations and statistical analysis are presented between the instruments used on the two separate aircraft platforms. These were found to be in good agreement giving a high degree of correlation for the ambient air studied. Any deviations from the correlations are accounted for in the estimated inaccuracies of the instruments. These results help to establish that the instruments aboard the separate aircraft are reliably able to measure the corresponding chemical species in the range of conditions sampled and that data collected by both aircraft can be co-ordinated for purposes of interpretation.

Unique in situ measurements of CO, O3, SO2, CH4, NO, NOx, NOy, VOC, CN, and rBC were carried out with the German Deutsches Zentrum für Luft‐ und Raumfahrt (DLR)‐Falcon aircraft in the central U.S. thunderstorms during the Deep Convective Clouds and Chemistry experiment in summer 2012. Fresh and aged anvil outflow (9–12 km) from supercells, mesoscale convective systems, mesoscale convective complexes, and squall lines were probed over Oklahoma, Texas, Colorado, and Kansas. For three case studies (30 May and 8 and 12 June) a combination of trace species, radar, lightning, and satellite information, as well as model results, were used to analyze and design schematics of major trace gas transport pathways within and in the vicinity of the probed thunderstorms. The impact of thunderstorms on the O3 composition in the upper troposphere/lower stratosphere (LS) region was analyzed. Overshooting cloud tops injected high amounts of biomass burning and lightning‐produced NOx emissions into the LS, in addition to low O3 mixing ratios from the lower troposphere. As a dynamical response, O3‐rich air from the LS was transported downward into the anvil and also surrounded the outflow. The ΔO3/ΔCO ratio was determined in the anvil outflow region. A pronounced in‐mixing of O3‐rich stratospheric air masses was observed in the outflow indicated by highly positive or even negative ΔO3/ΔCO ratios (+1.4 down to −3.9). Photochemical O3 production (ΔO3/ΔCO = +0.1) was found to be minor in the recently lofted pollution plumes. O3 mixing ratios within the aged anvil outflow were mainly enhanced due to dynamical processes.

Lightning is an important source of NO_x in the free troposphere, especially in the tropics, with high impact on ozone production. However, estimates of lightning NO_x (LNO_x) production efficiency (LNO_x per flash) are still quite uncertain.

In this study we present a systematic analysis of NO₂ column densities from SCIAMACHY measurements over active thunderstorms, as detected by the World-Wide Lightning Location Network (WWLLN), where the WWLLN detection efficiency was estimated using the flash climatology of the satellite lightning sensors LIS/OTD. Only events with high lightning activity are considered, where corrected WWLLN flash rate densities inside the satellite pixel within the last hour are above 1 /km²/h. For typical SCIAMACHY ground pixels of 30×60 km², this threshold corresponds to 1800 flashes over the last hour, which, for literature estimates of lightning NO_x production, should result in clearly enhanced NO₂ column densities.

From 2004–2008, we find 287 coincidences of SCIAMACHY measurements and high WWLLN flash rate densities. For some of these events, a clear enhancement of column densities of NO₂ could be observed, indeed. But overall, the measured column densities are below the expected values by more than one order of magnitude, and in most of the cases, no enhanced NO₂ could be found at all.

Our results are in contradiction to the currently accepted range of LNO_x production per flash of 15 (2–40)×10²⁵ molec/flash. This probably partly results from the specific conditions for the events under investigation, i.e. events of high lightning activity in the morning (local time) and mostly (for 162 out of 287 events) over ocean.

Within the detected coincidences, the highest NO₂ column densities were observed around the US Eastcoast. This might be partly due to interference with ground sources of NO_x being uplifted by the convective systems. However, it could also indicate that flashes in this region are particularly productive.

We conclude that current estimates of LNO_x production might be biased high for two reasons. First, we observe a high variability of NO₂ for coincident lightning events. This high variability can easily cause a publication bias, since studies reporting on high NO_x production have likely been published, while studies finding no or low amounts of NO_x might have been rejected as errorneous or not significant. Second, many estimates of LNO_x production in literature have been performed over the US, which is probably not representative for global lightning